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Bright single-nanocrystal upconversion at sub 0.5 W cm−2 irradiance via coupling to single nanocavity mode

Nature Photonics volume 17, pages 73–81 (2023)Cite this article

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Abstract

Lanthanide-doped nanocrystals have been actively pursued as anti-Stokes emitters in various contexts, including bioimaging, photovoltaics, catalysis, displays, anticounterfeiting, sensing and lasers. The success of these applications crucially relies on their high brightness under low excitation. To enhance their upconversion luminescence, researchers have improved the internal material properties of nanocrystals (their composition, doping, and crystal and surface structures) and, in parallel, engineered external optical responses using plasmonic couplings. However, despite impressive progress, upconversion brightness still falls short of what is required for applications, and a systematic understanding of plasmon-enhanced upconversion remains elusive. Here we report an important conceptual advance in understanding and demonstrate unprecedentedly bright upconversion of single nanocrystals via coupling to a single plasmonic nanocavity mode. We present in situ-controlled single-nanocrystal-level studies with unified internal and external treatment, and unambiguously experimentally demonstrate the phenomenon of plasmonic enhancement saturation. We show that the saturation is doping-dependent, and we report a 2.3 × 105-fold enhancement of upconversion luminescence. More importantly, we outline a new strategy to devise ultrabright upconversion nanomaterials and demonstrate that single sub-30-nm nanocrystals can provide up to 560 detected photons per second at an ultralow excitation intensity of 0.45 W cm−2. These findings help to establish the link between the optical physics and material science in lanthanide-doped nanocrystals and facilitate the engineering of optimal upconversion nanomaterials for various applications.

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Fig. 1: Principle and realization of controlled single-nanocrystal upconversion in a single plasmonic nanocavity mode.
Fig. 2: Nanocavity–UCNC composite featuring single-nanocrystal single-mode coupling.
Fig. 3: Experimental demonstration of the saturation of UCL enhancement.
Fig. 4: Ultrastrong UCL enhancement.
Fig. 5: Ultrabright UCL.

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Data availability

The data that support the findings of this study are available from the corresponding authors upon reasonable request.

Code availability

All codes used in this paper are available from the corresponding authors upon reasonable request.

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Acknowledgements

We gratefully acknowledge financial support from the National Natural Science Foundation of China (grant no. 11874166 to X.-W.C., 92150111 to X.-W.C., 62235006 to X.-W.C., 12004130 to J.T., 51972084 to G.C., 52272270 to G. C. and 51672061 to G.C.), the Fundamental Research Funds for the Central Universities, China (AUGA5710052614 to G.C.), the State Key Laboratory of Urban Water Resource and Environment (Harbin Institute of Technology; no. 2020DX10 to G.C.) and Huazhong University of Science and Technology (X.-W.C. and J.T.).

Author information

Authors and Affiliations

  1. School of Physics and Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan, China

    Yongjun Meng, Hong Li, Xia Feng, Qianyi Liang, Tianzi Ma, Jiahao Han, Jianwei Tang & Xue-Wen Chen

  2. MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering & Key Laboratory of Micro-systems and Micro-structures, Ministry of Education, Harbin Institute of Technology, Harbin, China

    Dingxin Huang, Feng Li & Guanying Chen

  3. Institute for Quantum Science and Engineering, Huazhong University of Science and Technology, Wuhan, China

    Jianwei Tang & Xue-Wen Chen

  4. Wuhan Institute of Quantum Technology, Wuhan, China

    Xue-Wen Chen

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Contributions

X.-W.C. conceived the research. X.-W.C., G.C. and J.T. designed the experiment. Y.M., J.T., X.F., T.M. and J.H. carried out the UCNC–nanocavity coupling experiment and optical measurements. D.H. and F.L. synthesized and characterized the UCNC samples under the guidance of G.C. J.T., X.-W.C., H.L., Q.L. and J.H. developed the theoretical model and performed numerical simulations. X.-W.C., G.C., J.T. and Y.M. discussed the results and analysed data. The paper was written by X.-W.C. and J.T., and comments were provided by Y.M. and G.C. The project was supervised by X.-W.C., J.T. and G.C.

Corresponding authors

Correspondence to Jianwei Tang, Guanying Chen or Xue-Wen Chen.

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Nature Photonics thanks Steven Chu, Aitzol García-Etxarri and Xiaogang Liu for their contribution to the peer review of this work.

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Supplementary Figs. 1–33, Discussion and Tables 1–5.

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Meng, Y., Huang, D., Li, H. et al. Bright single-nanocrystal upconversion at sub 0.5 W cm−2 irradiance via coupling to single nanocavity mode. Nat. Photon. 17, 73–81 (2023). https://doi.org/10.1038/s41566-022-01101-z

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